Related papers: Mixed quantum-classical dynamics using collective …

First-principles atomistic simulations are essential for understanding complex material phenomena but are fundamentally limited by their computational cost. While Machine Learning Interatomic Potentials (MLIPs) have drastically improved…

Accurate solution of the many-electron problem including correlations remains intractable except for few-electron systems. Describing interacting electrons as a superposition of independent electron configurations results in an apparent…

Event-driven molecular dynamics is a valuable tool in condensed and soft matter physics when particles can be modeled as hard objects or more generally if their interaction potential can be modeled in a stepwise fashion. Hard spheres model…

We extend ring-polymer molecular dynamics (RPMD) to allow for the direct simulation of general, electronically non-adiabatic chemical processes. The kinetically constrained (KC) RPMD method uses the imaginary-time path-integral…

Simulating electron-nucleus coupled dynamics poses a non-trivial challenge and an important problem in the investigation of ultrafast processes involving coupled electronic and vibrational dynamics. Because irreversibility of the system…

Classical molecular dynamics simulations have recently become a standard tool for the study of electrochemical systems. State-of-the-art approaches represent the electrodes as perfect conductors, modelling their responses to the charge…

In electronic structure theory, variational methods offer a valuable paradigm for approximating electronic ground states. However, for historical reasons, this principle is mostly restricted to model chemistries in pre-defined fixed basis…

We describe experimentally observed collective dynamics in colloidal suspensions of model hard-sphere particles using a modified mode coupling theory (MCT). This rescaled MCT is capable to describe quantitatively the wave-vector and…

We aim to automatize the identification of collective variables to simplify and speed up enhanced sampling simulations of conformational dynamics in biomolecules. We focus on anharmonic low-frequency vibrations that exhibit fluctuations on…

Most non-relativistic interacting quantum many-body systems, such as atomic and molecular ensembles or materials, are naturally described in terms of continuous-space Hamiltonians. The simulation of their ground-state properties on digital…

Multitime quantum correlation functions are central objects in physical science, offering a direct link between experimental observables and the dynamics of an underlying model. While experiments such as 2D spectroscopy and quantum control…

We present a universal expression for the electronic friction as felt by a set of classical nuclear degrees of freedom (DoF's) coupled to a manifold of quantum electronic DoF's; no assumptions are made regarding the nature of the electronic…

The exact nuclear time-dependent potential energy surface arises from the exact decomposition of electronic and nuclear motion, recently presented in [A. Abedi, N. T. Maitra, and E. K. U. Gross, Phys. Rev. Lett. 105, 123002 (2010)]. Such…

We developed a general framework for hybrid quantum-classical computing of molecular and periodic embedding approaches based on an orbital space separation of the fragment and environment degrees of freedom. We demonstrate its potential by…

We introduce an improved semiclassical dynamics approach to quantum vibrational spectroscopy. In this method, a harmonic-based phase space sampling is preliminarily driven toward non-harmonic quantization by slowly switching on the actual…

Electronic nearsightedness is one of the fundamental principles governing the behavior of condensed matter and supporting its description in terms of local entities such as chemical bonds. Locality also underlies the tremendous success of…

In classical computational chemistry, the coupled-cluster ansatz is one of the most commonly used $ab~initio$ methods, which is critically limited by its non-unitary nature. The unitary modification as an ideal solution to the problem is,…

We present a new approach for the two-temperature molecular dynamics (MD) model for coupled simulations of electronic and phonon heat conduction in nanoscale systems. The proposed method uses a master equation to perform heat conduction of…

We present our successful implementation of the quantum electrodynamics coupled-cluster method with single and double excitations (QED-CCSD) for electronic and bosonic amplitudes, covering both individual and mixed excitation processes…

Constant potential method molecular dynamics simulation (CPM MD) enables the accurate modelling of atomistic electrode charges when studying the electrode-electrolyte interface at the nanoscale. Here we extend the theoretical framework of…